Mechanistic insights into lytic polysaccharide monooxygenases: an integrated structure/spectroscopy study

含金属的酶在生物学的整个范围内执行关键的生化功能。它们也存在于许多日常产品中，如洗衣粉和清洁产品。此外，这些类型的酶在工业（例如造纸）中使用非常广泛。因此，我们对它们的详细生物化学和化学的任何了解都具有重大的社会效益。在大多数这些酶中，金属离子是酶活性位点的基本特征，并且在许多情况下，活性位点处的金属是过渡金属，例如Fe、Mn、Cu。这种类型的活性位点的独特之处在于，它们通常能够进行“非凡”的化学反应，其中通常不反应的底物的转化被催化。这也许并不比自然界部署的将丰富的生物质（例如木材，纤维素和甲烷）转化为生物有价值的产品的酶更真实，其中含金属的酶进行许多关键的转化步骤。因此，这些酶的知识和利用对于无数行业是必不可少的，其中最引人注目的可能是新生的第二代生物燃料行业，其中通过生物质原料的酶促降解将富含柠檬酸的生物质转化为生物乙醇。事实上，这个项目集中在一个全新的酶称为溶解性多糖单加氧酶，其中含有铜。这些酶被证明是我们将废弃植物物质（例如树叶和秸秆）转化为生物燃料的关键因素。事实上，这些酶是世界上几个新的生物精炼厂开放的部分原因，这些生物精炼厂能够将草转化为生物乙醇。因此，该项目旨在详细了解酶的工作原理，并找到提高其转化能力的方法。

Metal-containing enzymes perform critical biochemical functions across the full breadth of biology. They are also found in many everyday products such as washing powders and cleaning products. Furthermore, these types of enzymes are used very widely by industry (e.g. paper manufacture). Therefore, any insight we can gain into their detailed biochemistry and chemistry has significant societal benefits. In most of these enzymes the metal ion is an essential feature of the enzyme's active site, and in many cases the metal(s) at the active site is/are (a) transition metals, e.g. Fe, Mn, Cu. What is distinctive about such types of active site is that they are often capable of 'extraordinary' chemistry in which the conversion of normally unreactive substrates is catalysed. This is perhaps no truer than in the enzymes which Nature deploys to convert abundant biomass (e.g. wood, cellulose and methane respectively) through to bio-valuable products, where metal-containing enzymes carry out many of the key conversion steps. As such, knowledge of and utilisation of these enzymes is essential for myriad industries, perhaps the most conspicuous of which is the nascent second-generation biofuel industry in which recalcitrant and abundant biomass is converted through to bioethanol through enzymatic degradation of the biomass feedstock. Indeed this projects concentrates on a brand new set of enzymes called lytic polysaccharide monooxygenase which contain copper. These enzymes are proving to be key factors in our ability to convert waste plant matter (e.g. leaves and stalks) through to biofuel. In fact, these enzymes are part of the reason why several new biorefineries have opened-up around the world which are able to convert grasses through to bioethanol. This project, therefore, seeks to understand in detail how the enzymes work and also to find ways to improve their conversion capabilities.